Abstract
The indirect attack mechanism of O-1(2) on electron donors (ED) provides a new idea for improving photo -production of H2O2 (PHO). Inspired by this, we constructed oxygen activation and .O2- oxidation sites in g-C3N4 to promote the 100% conversion of .O2- to O-1(2) for PHO. Based on experimental data, we unexpect-edly discovered the coordinated regulation of spin polarization and water bridge (CRSPWB) in H2O2 generation reaction by theoretical calculation. The O-1(2) can react with ED to produce H2O2 in the most favourable way under the CRSPWB, which modifies the electronic structures of O-1(2) and ED to maximize the interaction between them. Besides, water bridge indirectly enhances the oxidation effect of O-1(2) on ED. Thus, corresponding reaction barrier for H2O2 generation is reduced to as low as-0.07 eV. This work pro-vides in-depth insights into the attack behavior of O-1(2) in H2O2 generation and brand-new guidance for improving PHO.(c) 2022 Elsevier Inc. All rights reserved.